CHARACTERISTICS OF O-O BONDS IN $O_{2}, O_{3},HO_{2}(^{2}A'',^{2}A'), H_{2}O_{2}$ AND $H_{2}O_{3}$

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1973

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Ohio State University

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The nature of the interoxygen bond in $O_{2}, O_{3}, HO_{2}(^{2}A^{\prime\prime}, ^{2}A^{\prime}), H_{2}O_{2}$ and $H_{2}O_{3}$ has been investigated on the basis of ab initio (LCAO-MO) and experimental force constants, bond lengths, and energies. Certain anomalous results for the calculated $HO_{2}$ force constants prompted an analysis of the sensitivity of the above properties to various types of contracated Gaussian Type Orbitals (GTOs); the discussed results are based on an extended sp set of GTOs (in some cases supplemented by d orbitals). The order of decreasing calculated force constants and increasing bond lengths for the O-O bond is $O_{2}, O_{3}, HO_{2}(^{2}A^{\prime\prime}), H_{2}O_{3}, H_{2}O_{2}$ and $HO_{2}(^{2}A^{\prime})$. This ordering is related to available experimental data and is also analyzed in terms of partial O-O double bond character. Relative O-O bond energies of $HO_{2}, H_{2}O_{2}$ and $H_{2}O_{3}$ are compared based on appropriate balanced chemical equations. With the sp basis, bond lengths and bond angles for the ground $(^{2}A^{\prime\prime})$ and the first excited state $(^{2}A^{\prime})$ of $HO_{2}$ have been determined to be 1.363 \AA, $107.9^{\circ}$ and 1.437 \AA, $104.8^{\circ}$ respectiavely. The adiabatic and vertical excitation energies between these two states range between 11 and 23 keal/mole. In summary, it is demonstrated that the range of properties in the set of molecules studied is adequately described by a consistent and sufficiently flexible level of calculation.

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Author Institution: Department of Chemistry, Brookhaven National

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